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yexuqing木虫之王 (文学泰斗)
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[交流]
液电池TEM中带电固液界面的原子动力学
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液电池TEM中带电固液界面的原子动力学 ▲ 作者：Qiubo Zhang, Zhigang Song, Xianhu Sun, Yang Liu, Jiawei Wan, Sophia B. Betzler, Qi Zheng, Junyi Shangguan, Karen C. Bustillo, Peter Ercius, Prineha Na ▲ 链接： https://www.nature.com/articles/s41586-024-07479-w ▲ 摘要： 带电固液界面在与能源、生物和地球化学相关的各种电化学过程中起着关键作用。带电界面上的电子和质量传递可能导致结构改变，从而显著影响反应途径。例如，电催化剂在反应过程中的表面重组会对催化机理和反应产物产生实质性的影响。 尽管它很重要，但直接探测电偏置下固液界面的原子动力学是具有挑战性的，因为它被埋在液体电解质中，而且目前通过液体进行原位成像的技术空间分辨率有限。研究者开发了用于透射电子显微镜（TEM）的先进聚合物电化学液体电池，能够直接监测铜催化二氧化碳电还原反应（CO2ERs）过程中ESLIs的原子动力学。 研究者观察揭示了一个波动的液体状无定形界面。它发生可逆的晶—非晶结构转变，并沿通电铜表面流动，从而通过界面层介导结晶铜表面重构和质量损失。实时观察和理论计算的结合揭示了由电荷激活的电解质表面反应引起的非晶化介导的重组机制。通过利用原位成像能力，该的结果为探索原子动力学及其在涉及ESLIs的广泛系统中的影响提供了许多机会。 ▲ Abstract： Electrified solid–liquid interfaces (ESLIs) play a key role in various electrochemical processes relevant to energy, biology and geochemistry. The electron and mass transport at the electrified interfaces may result in structural modifications that markedly influence the reaction pathways. For example, electrocatalyst surface restructuring during reactions can substantially affect the catalysis mechanisms and reaction products. Despite its importance, direct probing the atomic dynamics of solid–liquid interfaces under electric biasing is challenging owing to the nature of being buried in liquid electrolytes and the limited spatial resolution of current techniques for in situ imaging through liquids. Here, with our development of advanced polymer electrochemical liquid cells for transmission electron microscopy (TEM), we are able to directly monitor the atomic dynamics of ESLIs during copper (Cu)-catalysed CO2 electroreduction reactions (CO2ERs). Our observation reveals a fluctuating liquid-like amorphous interphase. It undergoes reversible crystalline–amorphous structural transformations and flows along the electrified Cu surface, thus mediating the crystalline Cu surface restructuring and mass loss through the interphase layer. The combination of real-time observation and theoretical calculations unveils an amorphization-mediated restructuring mechanism resulting from charge-activated surface reactions with the electrolyte. Our results open many opportunities to explore the atomic dynamics and its impact in broad systems involving ESLIs by taking advantage of the in situ imaging capability. |
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